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Electrochemical and Electrogenerated Chemiluminescent Studies of a Trinuclear Complex, [((phen)2Ru(dpp))2RhCl2]5+, and Its Interactions with Calf Thymus DNA

Wang, Shijun (author)
Milam, Jenifer (author)
Ohlin, C. Andre (author)
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Rambaran, Varma H. (author)
Clark, Eva (author)
Ward, Woodrow (author)
Seymour, Luke (author)
Casey, William H. (author)
Holder, Alvin A. (author)
Miao, Wujian (author)
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2009-04-09
2009
English.
In: Analytical Chemistry. - : American Chemical Society (ACS). - 0003-2700 .- 1520-6882. ; 81:10, s. 4068-4075
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http://dx.doi.org/10...
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https://urn.kb.se/re...
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  • Journal article (peer-reviewed)
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  • The electrochemical behavior of a trinuclear ruthenium(II)-containing complex, [((phen)2Ru(dpp))2RhCl2]5+ (where phen = 1,10-phenanthroline, dpp = 2,3-bis(2-pyridyl)pyrazine), was studied in acetonitrile (MeCN) and aqueous solutions. In MeCN containing 0.10 M tetra-n-butylammonium perchlorate (TBAP), the complex displayed a reversible, overlapping RuII/III redox process with E1/2 = +1.21 V vs Ag/Ag+ (10 mM), an irreversible reduction of RhIII/I at −0.73 V vs Ag/Ag+, and two quasi-reversible dpp/dpp− couples with E1/2 = −1.11 and −1.36 V vs Ag/Ag+ at a Pt electrode with a scan rate of 50 mV s−1. In 0.20 M Tris buffer solution (pH 7.4), an irreversible, overlapping RuII/III oxidation at +1.48 V vs Ag/AgCl (3 M KCl), and an irreversible reduction of RhIII/II at −0.78 V vs Ag/AgCl were observed at a glassy carbon electrode with a scan rate of 50 mV/s. Investigations on the electrogenerated chemiluminescence (ECL) of the complex revealed that 2-(dibutylamino) ethanol (DBAE) was superior to tri-n-propylamine (TPrA) as an ECL coreactant within their entire concentration range of 10−100 mM in MeCN, and in aqueous media, as low as 1.0 nM of the complex can be detected using TPrA coreactant ECL. A maximum ECL emission of 640 nm, which is about 55 nm blue shift to its fluorescence, was observed in MeCN with DBAE as a coreactant. Interactions of the complex with calf thymus DNA (ctDNA) were conducted with a flow-cell based quartz-crystal microbalance, and a binding constant of 2.5 × 105 M−1 was calculated on the basis of the Langmuir isotherm equation.

Subject headings

NATURVETENSKAP  -- Kemi -- Analytisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Analytical Chemistry (hsv//eng)
NATURVETENSKAP  -- Kemi -- Oorganisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Inorganic Chemistry (hsv//eng)

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